Femtosecond Polarization Switching in the Crystal of a [CrCo] Dinuclear Complex
Capability to control macroscopic molecular properties with external stimuli offers the possibility to exploit molecules as switching devices of various types. However, application of such molecular‐level switching has often been limited by its speed and thus efficiency. Herein, we demonstrate ultra...
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Veröffentlicht in: | Angewandte Chemie International Edition 2020-09, Vol.59 (37), p.15865-15869 |
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description | Capability to control macroscopic molecular properties with external stimuli offers the possibility to exploit molecules as switching devices of various types. However, application of such molecular‐level switching has often been limited by its speed and thus efficiency. Herein, we demonstrate ultrafast, photoinduced polarization switching in the crystal of a [CrCo] dinuclear complex by ultrafast pump–probe spectroscopy in the visible and mid‐infrared regions. The photoinduced polarization switching was found to have a time constant of 280 fs, which makes the [CrCo] complex crystal the fastest polarization‐switching material realized using the metastable state. Moreover, the pump–probe data in the visible region reveal the pronounced appearance of coherent nuclear wavepacket motion with a frequency as low as 22 cm−1, which we attribute to a lattice vibrational mode. The pronounced non‐Condon effect for its resonance Raman enhancement implies that this mode couples the relevant electronic states, thereby facilitating the ultrafast polarization switching.
Full speed ahead: Ultrafast spectroscopy revealed that photoinduced polarization switching in the crystal of a [CrCo] dinuclear complex proceeded with a time constant of 280 fs (see picture; LT/HT=low‐/high‐temperature, dhsq/dhbq= deprotonated dihydroxysemi‐/benzoquinone). The pronounced appearance of a low‐frequency coherent vibration and its mechanism suggest that the corresponding excited‐state vibrational mode facilitates the polarization switching. |
doi_str_mv | 10.1002/anie.202004583 |
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Full speed ahead: Ultrafast spectroscopy revealed that photoinduced polarization switching in the crystal of a [CrCo] dinuclear complex proceeded with a time constant of 280 fs (see picture; LT/HT=low‐/high‐temperature, dhsq/dhbq= deprotonated dihydroxysemi‐/benzoquinone). The pronounced appearance of a low‐frequency coherent vibration and its mechanism suggest that the corresponding excited‐state vibrational mode facilitates the polarization switching.</description><edition>International ed. in English</edition><identifier>ISSN: 1433-7851</identifier><identifier>EISSN: 1521-3773</identifier><identifier>DOI: 10.1002/anie.202004583</identifier><language>eng</language><publisher>Weinheim: Wiley Subscription Services, Inc</publisher><subject>Crystals ; Electron states ; External stimuli ; heterometallic complexes ; Metastable state ; Polarization ; polarization switching ; Spectroscopy ; Switching ; Time constant ; time-resolved spectroscopy ; ultrafast dynamics ; vibrational spectroscopy ; Wave packets</subject><ispartof>Angewandte Chemie International Edition, 2020-09, Vol.59 (37), p.15865-15869</ispartof><rights>2020 Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim</rights><rights>2020 Wiley‐VCH GmbH</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c4533-935fa351fe2e9fe05b663f34ad9e8fb9e126efed33513edca8d8904ce5b375923</citedby><cites>FETCH-LOGICAL-c4533-935fa351fe2e9fe05b663f34ad9e8fb9e126efed33513edca8d8904ce5b375923</cites><orcidid>0000-0002-6340-8535 ; 0000-0003-3663-5991 ; 0000-0001-5666-3880 ; 0000-0003-2256-8628 ; 0000-0002-5269-0598 ; 0000-0002-4646-1318</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fanie.202004583$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fanie.202004583$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,776,780,1411,27901,27902,45550,45551</link.rule.ids></links><search><creatorcontrib>Kuramochi, Hikaru</creatorcontrib><creatorcontrib>Aoyama, Genki</creatorcontrib><creatorcontrib>Okajima, Hajime</creatorcontrib><creatorcontrib>Sakamoto, Akira</creatorcontrib><creatorcontrib>Kanegawa, Shinji</creatorcontrib><creatorcontrib>Sato, Osamu</creatorcontrib><creatorcontrib>Takeuchi, Satoshi</creatorcontrib><creatorcontrib>Tahara, Tahei</creatorcontrib><title>Femtosecond Polarization Switching in the Crystal of a [CrCo] Dinuclear Complex</title><title>Angewandte Chemie International Edition</title><description>Capability to control macroscopic molecular properties with external stimuli offers the possibility to exploit molecules as switching devices of various types. However, application of such molecular‐level switching has often been limited by its speed and thus efficiency. Herein, we demonstrate ultrafast, photoinduced polarization switching in the crystal of a [CrCo] dinuclear complex by ultrafast pump–probe spectroscopy in the visible and mid‐infrared regions. The photoinduced polarization switching was found to have a time constant of 280 fs, which makes the [CrCo] complex crystal the fastest polarization‐switching material realized using the metastable state. Moreover, the pump–probe data in the visible region reveal the pronounced appearance of coherent nuclear wavepacket motion with a frequency as low as 22 cm−1, which we attribute to a lattice vibrational mode. The pronounced non‐Condon effect for its resonance Raman enhancement implies that this mode couples the relevant electronic states, thereby facilitating the ultrafast polarization switching.
Full speed ahead: Ultrafast spectroscopy revealed that photoinduced polarization switching in the crystal of a [CrCo] dinuclear complex proceeded with a time constant of 280 fs (see picture; LT/HT=low‐/high‐temperature, dhsq/dhbq= deprotonated dihydroxysemi‐/benzoquinone). The pronounced appearance of a low‐frequency coherent vibration and its mechanism suggest that the corresponding excited‐state vibrational mode facilitates the polarization switching.</description><subject>Crystals</subject><subject>Electron states</subject><subject>External stimuli</subject><subject>heterometallic complexes</subject><subject>Metastable state</subject><subject>Polarization</subject><subject>polarization switching</subject><subject>Spectroscopy</subject><subject>Switching</subject><subject>Time constant</subject><subject>time-resolved spectroscopy</subject><subject>ultrafast dynamics</subject><subject>vibrational spectroscopy</subject><subject>Wave packets</subject><issn>1433-7851</issn><issn>1521-3773</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><recordid>eNqFkE1LAzEQhoMoWKtXzwEvXrYmm2Q_jmVttVBUUE8iS5qd2JTdTU12qfXXm1JR8OJp5vA8My8vQueUjCgh8ZVsDYxiEhPCRcYO0ICKmEYsTdlh2DljUZoJeoxOvF8FPstIMkD3U2g660HZtsIPtpbOfMrO2BY_bkynlqZ9w6bF3RJw4ba-kzW2Gkv8UrjCvuJr0_aqBulwYZt1DR-n6EjL2sPZ9xyi5-nkqbiN5vc3s2I8jxQXIUnOhJZMUA0x5BqIWCQJ04zLKodML3KgcQIaKhYYBpWSWZXlhCsQC5aKPGZDdLm_u3b2vQfflY3xCupatmB7X8acCEYYDc-G6OIPurK9a0O6QHHCeUooCdRoTylnvXegy7UzjXTbkpJy12-567f86TcI-V7YmBq2_9Dl-G42-XW_AJM-fjg</recordid><startdate>20200907</startdate><enddate>20200907</enddate><creator>Kuramochi, Hikaru</creator><creator>Aoyama, Genki</creator><creator>Okajima, Hajime</creator><creator>Sakamoto, Akira</creator><creator>Kanegawa, Shinji</creator><creator>Sato, Osamu</creator><creator>Takeuchi, Satoshi</creator><creator>Tahara, Tahei</creator><general>Wiley Subscription Services, Inc</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7TM</scope><scope>K9.</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0002-6340-8535</orcidid><orcidid>https://orcid.org/0000-0003-3663-5991</orcidid><orcidid>https://orcid.org/0000-0001-5666-3880</orcidid><orcidid>https://orcid.org/0000-0003-2256-8628</orcidid><orcidid>https://orcid.org/0000-0002-5269-0598</orcidid><orcidid>https://orcid.org/0000-0002-4646-1318</orcidid></search><sort><creationdate>20200907</creationdate><title>Femtosecond Polarization Switching in the Crystal of a [CrCo] Dinuclear Complex</title><author>Kuramochi, Hikaru ; Aoyama, Genki ; Okajima, Hajime ; Sakamoto, Akira ; Kanegawa, Shinji ; Sato, Osamu ; Takeuchi, Satoshi ; Tahara, Tahei</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c4533-935fa351fe2e9fe05b663f34ad9e8fb9e126efed33513edca8d8904ce5b375923</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><topic>Crystals</topic><topic>Electron states</topic><topic>External stimuli</topic><topic>heterometallic complexes</topic><topic>Metastable state</topic><topic>Polarization</topic><topic>polarization switching</topic><topic>Spectroscopy</topic><topic>Switching</topic><topic>Time constant</topic><topic>time-resolved spectroscopy</topic><topic>ultrafast dynamics</topic><topic>vibrational spectroscopy</topic><topic>Wave packets</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Kuramochi, Hikaru</creatorcontrib><creatorcontrib>Aoyama, Genki</creatorcontrib><creatorcontrib>Okajima, Hajime</creatorcontrib><creatorcontrib>Sakamoto, Akira</creatorcontrib><creatorcontrib>Kanegawa, Shinji</creatorcontrib><creatorcontrib>Sato, Osamu</creatorcontrib><creatorcontrib>Takeuchi, Satoshi</creatorcontrib><creatorcontrib>Tahara, Tahei</creatorcontrib><collection>CrossRef</collection><collection>Nucleic Acids Abstracts</collection><collection>ProQuest Health & Medical Complete (Alumni)</collection><collection>MEDLINE - Academic</collection><jtitle>Angewandte Chemie International Edition</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Kuramochi, Hikaru</au><au>Aoyama, Genki</au><au>Okajima, Hajime</au><au>Sakamoto, Akira</au><au>Kanegawa, Shinji</au><au>Sato, Osamu</au><au>Takeuchi, Satoshi</au><au>Tahara, Tahei</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Femtosecond Polarization Switching in the Crystal of a [CrCo] Dinuclear Complex</atitle><jtitle>Angewandte Chemie International Edition</jtitle><date>2020-09-07</date><risdate>2020</risdate><volume>59</volume><issue>37</issue><spage>15865</spage><epage>15869</epage><pages>15865-15869</pages><issn>1433-7851</issn><eissn>1521-3773</eissn><abstract>Capability to control macroscopic molecular properties with external stimuli offers the possibility to exploit molecules as switching devices of various types. However, application of such molecular‐level switching has often been limited by its speed and thus efficiency. Herein, we demonstrate ultrafast, photoinduced polarization switching in the crystal of a [CrCo] dinuclear complex by ultrafast pump–probe spectroscopy in the visible and mid‐infrared regions. The photoinduced polarization switching was found to have a time constant of 280 fs, which makes the [CrCo] complex crystal the fastest polarization‐switching material realized using the metastable state. Moreover, the pump–probe data in the visible region reveal the pronounced appearance of coherent nuclear wavepacket motion with a frequency as low as 22 cm−1, which we attribute to a lattice vibrational mode. The pronounced non‐Condon effect for its resonance Raman enhancement implies that this mode couples the relevant electronic states, thereby facilitating the ultrafast polarization switching.
Full speed ahead: Ultrafast spectroscopy revealed that photoinduced polarization switching in the crystal of a [CrCo] dinuclear complex proceeded with a time constant of 280 fs (see picture; LT/HT=low‐/high‐temperature, dhsq/dhbq= deprotonated dihydroxysemi‐/benzoquinone). The pronounced appearance of a low‐frequency coherent vibration and its mechanism suggest that the corresponding excited‐state vibrational mode facilitates the polarization switching.</abstract><cop>Weinheim</cop><pub>Wiley Subscription Services, Inc</pub><doi>10.1002/anie.202004583</doi><tpages>5</tpages><edition>International ed. in English</edition><orcidid>https://orcid.org/0000-0002-6340-8535</orcidid><orcidid>https://orcid.org/0000-0003-3663-5991</orcidid><orcidid>https://orcid.org/0000-0001-5666-3880</orcidid><orcidid>https://orcid.org/0000-0003-2256-8628</orcidid><orcidid>https://orcid.org/0000-0002-5269-0598</orcidid><orcidid>https://orcid.org/0000-0002-4646-1318</orcidid></addata></record> |
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subjects | Crystals Electron states External stimuli heterometallic complexes Metastable state Polarization polarization switching Spectroscopy Switching Time constant time-resolved spectroscopy ultrafast dynamics vibrational spectroscopy Wave packets |
title | Femtosecond Polarization Switching in the Crystal of a [CrCo] Dinuclear Complex |
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